Radioactive iodine is one of the main substances existed in nuclear wastes. It can quickly diffuse into the atmosphere causing great harm to environment and human health. Therefore, how to capture radioactive iodine efficiently has become a research hotspot. Herein, a covalent organic framework (COF) material (COF-1) has been synthesized by aldimine condensation reaction using the 1,3,5-triazine structure compound and isophthalaldehyde as starting materials. The nitrogen-rich COF-1 possesses medium specific surface area (321.78 m 2 /g), a pore diameter of 1.98 nm and relatively regular layered stack structure, which provide good conditions for iodine adsorption ability. The maximum iodine uptake of COF-1 is 2647 mg/g, which is higher than most iodine adsorbents reported. Subsequently, the release of iodine can be achieved in methanol indicating the iodine adsorption of COF-1 is a reversible process. It is also shown that COF-1 can be recycled. These characteristics maybe make COF-1 materials as a good iodine capturer in practical applications.Nuclear energy is a very important source of energy and its use will inevitably produce waste materials containing radioactive materials, of which the radionuclides 129 I and 131 I are the main components. Their half-lives are 15.7 million years and 8 days respectively. They can diffuse into the air quickly and exist for an extremely long time. 1 Radioactive iodine can also enter the human body through water, food, etc, and cause serious harm to environment and human health. 2,3 Thus, the research on iodine adsorption has attracted broad interests. The earliest iodine adsorbents were mainly inorganic adsorption materials, activated carbon, 4 zeolite 5 etc. Recent studies have shown that the large pore size and strong affinity for iodine are important factors of affecting the iodine adsorption performance. 6 Therefore, porous materials such as metal-organic framework (MOF), 7 conjugated microporous polymers 8 have also been used for